燃料電池和金屬-空氣電池作為能源轉(zhuǎn)換裝置具有較高的能量轉(zhuǎn)換率、高能量密度以及低環(huán)境影響等優(yōu)點(diǎn)。氧還原反應(yīng)是這些能源轉(zhuǎn)換裝置中非常關(guān)鍵的一個(gè)反應(yīng)。開(kāi)發(fā)高性能的氧還原電催化劑對(duì)于實(shí)現(xiàn)這些裝置得規(guī)模化應(yīng)用非常重要。氧還原催化劑的電催化活性常常與其比表面積、晶面結(jié)構(gòu)、導(dǎo)電性等因素有關(guān)。因此通過(guò)優(yōu)化這些因素實(shí)現(xiàn)氧還原催化劑的活性提升是非�？尚械摹＝陙�(lái),金屬有機(jī)框架(MOFs)由于其具有高比表面積、均勻的孔隙分布和可調(diào)控的機(jī)能等優(yōu)勢(shì),已廣泛應(yīng)用作為前驅(qū)體制備雜原子修飾的多孔碳材料。不僅如此,應(yīng)用該類材料所制備的催化劑相比于其他前驅(qū)體制備得到的催化劑具有更高的催化活性。因此,本文中,我們應(yīng)用MOFs制備了多種雜原子(N,Fe,Mn,和Co)摻雜的具有高比表面積的多孔碳材料,并研究了這些催化劑在堿性溶液和酸性溶液中的電催化氧還原性能。由于MOFs獨(dú)特的結(jié)構(gòu),所制備的碳基催化劑不僅具有大量的活性位點(diǎn),而且其良好的介孔結(jié)構(gòu)為物質(zhì)的傳輸提供大量的通道。此外,本文重點(diǎn)探討了不同的摻雜金屬原子對(duì)MOFs衍生的過(guò)渡金屬摻雜碳催化劑活性的影響,并且總結(jié)了不同金屬影響催化活性的規(guī)律。進(jìn)一步地,我們合成了二元金屬/三...

【文章頁(yè)數(shù)】：115 頁(yè)

【學(xué)位級(jí)別】：博士

【文章目錄】：
中文摘要
ABSTRACT
1 INTRODUCTION
    1.1 FOSSIL FUELS AND THE NEED FOR RESEARCH INTO ALTERNATIVES
    1.2 THE CURRENT ELECTROCHEMICAL DEVICES
    1.3 OXYGEN REDUCTION ELECTROCATALYSIS – A CHALLENGE
    1.4 NON-Pt CATALYSTS
        1.4.1 Metal Free Carbon Catalysts
        1.4.2 Transition Metal–Nitrogen–Carbon Catalysts
        1.4.3 The Mechanisms for ORR
    1.5 NANO-STRUCTURES DERIVED FROM MOFS
    1.6 SCOPE AND OBJECTIVE
2 EXPERIMENTAL METHODS AND CHARACTERIZATION TECHNIQUES
    2.1 EXPERIMENTAL METHODS
        2.1.1 General considerations about MOF mediated synthesis
        2.1.2 Cobalt (Co)-MOFMS
        2.1.3 Zinc (Zn)-MOFMS
    2.2 CHARACTERIZATION TECHNIQUES
        2.2.1 Scanning Electron Microscopy (SEM)
        2.2.2 Transmission Electron Microscopy (TEM)
        2.2.3 Brunauer, Emmet, Teller Adsorption Isotherm (BET)
        2.2.4 X-Ray Photoelectron Spectroscopy (XPS)
        2.2.5 X-Ray Diffraction (XRD)
    2.3 ELECTROCATALYSIS FOR ORR
        2.3.1 Rotating Ring Disk Electrode (RRDE) and Potentiostat
        2.3.2 Half-cell
        2.3.3 Linear Sweep Voltammetry (LSV)
        2.3.4 Cyclic Voltammetry (CV)
        2.3.5 Ring current analysis
3 REPERCUSSION AND DATA ANALYSIS
    3.1 SYNTHESIS OF ORR ELECTROCATALYST FROM ZIF-8 AND ZIF-67 AND BIMETALIC
        3.1.1 Introduction
        3.1.2 Experimental Section
        3.1.3 Results and Discussions
        3.1.4 Electrocatalytic Activity
        3.1.5 Conclusion
    3.2 DESIGN AND SYNTHESIS OF Mn/ZIF-8 DERIVED POLYHEDRONS ENRICHED WITH Mn-OXIDE ACTIVE-CENTRES
        3.2.1 Introduction
        3.2.2 Experimental
        3.2.3 Structural Characterization and Catalytic Activity
        3.2.4 ORR Electrocatalytic Acitvity
        3.2.5 Conclusion
    3.3 Fe/Zn-DICYANOIMIDAZOLATE FRAMEWORK DERIVED CARBON MICROSTRUCTURES FOR ORR
        3.3.1 Introduction
        3.3.2 Experimental
        3.3.3 Detailed Results and Discussion
    3.4 Fe-DOPED ZIF-67/8 MOFS DERIVED ORR CATALYSTS
        3.4.1 Experimental
        3.4.2 Structure Analysis and Electrocatalytic Activity
    3.5 INFLUENCE OF Mn DOPING ON MESOPOROUS CO-N/C DERIVED FROM ZIF
        3.5.1 Introduction
        3.5.2 Experimental
        3.5.3 Characterizations and Electrocatalytic Activity
4 CONCLUSION AND OUTLOOK
ACKNOWLEDGEMENTS
REFERENCES AND NOTES
PUBLICATIONS



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